The asymmetrical distribution of specific proteins on both sides the cell membrane, which is used to adjust the ion permeability, is magical inside the body of a living creature. These porous membrane materials with asymmetric micro/nanochannels are very common and important in both nature and artificial materials. Inspired by this, the construction of intelligent nanodevices with multifunctional properties is urgent and significant. Here a general strategy based on simultaneous chemical polymerization reactions in both sides of an anodic aluminum oxide (AAO) membrane is reported, combining with atom transfer radical polymerization (ATRP), dopamine self-polymerization (DOP-SP) and ring-opening metathesis polymerization (ROMP) technologies, to form various asymmetric membranes in the AAO nanochannels. By this method, double hydrophilic poly(3-sulfopropyl methacrylate potassium salt)@poly(2-(methacryloyloxy)ethyl-methylammonium chloride) (PSPMA@PMETAC), temperature and pH double responsive poly(N-isopropylacrylamide)@poly(dimethylamino)ethyl methacrylate (PNIPAM@PDMAEMA), and hydrophilic/hydrophobic poly(3-sulfopropyl methacrylate potassium salt)@poly(hydrophobic pentadecafluorooctyl-5-norbornene-2-carboxylate) (PSPMA@PNCA-F15) polymer brushes-modified asymmetrical AAO nanochannel array membranes were successfully prepared. Moreover, after the in situ ion exchange and reduction reaction of the double hydrophilic PSPMA@PMETAC membrane, we prepared polymer brushes-stabilized Au–Pd asymmetrically-modified AAO nanochannels, showing excellent flow-through catalysis.